Initial formaldehyde generation as a predictive marker for long-term stability of Ni-rich Li-ion batteries under abusive conditions

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Electrolyte decomposition significantly impacts the long-term stability of Li-ion batteries, generating liquid and gaseous byproducts. This study focuses on formaldehyde formation, a critical byproduct from CO2 reduction in Ni-rich Li-ion batteries. Through experimental and computational analyses, formaldehyde emerges from carbonate-based electrolyte decomposition. Examining overcharge, over-discharge, and fast charging conditions, formaldehyde concentration sharply increases under overcharge, indicating severe electrolyte breakdown, while over-discharge shows a gradual rise. Fast charging similarly elevates formaldehyde levels, underscoring the link between electrolyte decomposition and abusive conditions. Importantly, this research proposes utilizing formaldehyde concentration from the initial cycle as a predictive marker for assessing long-term Ni-rich Li-ion battery stability trends. Elevated initial formaldehyde indicates potential capacity fade and accelerated degradation, enabling proactive mitigation strategies. The study elucidates mechanisms governing formaldehyde formation, providing a foundation for developing electrolyte formulations and electrode materials with enhanced decomposition resistance and improved stability. This investigation contributes to the fundamental understanding of electrolyte decomposition in Ni-rich Li-ion batteries and presents a novel approach to predicting long-term performance based on initial formaldehyde measurements, advancing high-performance and reliable energy storage solutions.